Time-resolved imaging of atoms and molecules in laser-produced uranium plasmas

Kautz, Elizabeth J.; Skrodzki, Patrick J.; Burger, Milos; Bernacki, Bruce E.; Jovanovic, Igor; Phillips, Mark C.; Harilal, Sivanandan S.

doi:10.1039/C9JA00228F

Time-resolved imaging of atoms and molecules in laser-produced uranium plasmas

Journal Article · Fri Nov 01 00:00:00 EDT 2019 · Journal of Analytical Atomic Spectrometry

DOI:https://doi.org/10.1039/C9JA00228F· OSTI ID:1574887

Kautz, Elizabeth J. ^[1]; Skrodzki, Patrick J. ^[2]; Burger, Milos ^[2]; Bernacki, Bruce E. ^[1]; Jovanovic, Igor ^[3]; Phillips, Mark C. ^[4]; ^[1]

BATTELLE (PACIFIC NW LAB)
UNIVERSITY OF MICHIGAN
University of Michigan
UNIVERSITY PROGRAMS

Gas-phase oxidation of uranium (U), plume chemistry, and its impact on optical emission features of the uranium plasma are investigated. Plasmas were produced via nanosecond laser ablation of a natural uranium target in a chamber where uranium oxidation was controlled by varying the oxygen partial pressure within argon cover gas. Monochromatic imaging of uranium atoms and monoxide molecules was performed using narrowband optical filters, which clearly reveals the spatio-temporal evolution of these species in the plasma. Uranium oxides are found to be formed at the plasma edges, where lower temperatures favor molecular recombination. Segregation between the distribution of uranium atoms and monoxide species is observed at later times of plasma evolution, and is more apparent at lower oxygen partial pressures. At higher oxygen partial pressures, significant variation in plume morphology is noticed for UO species, which is attributed to higher rate of oxide (UxOy) formation at the plume edges. The monochromatic images of U atoms and molecules and corresponding spectral features at various oxygen partial pressures presented here provide a unique insight into gas-phase, high-temperature uranium oxidation, and its chemistry and have implications for a wide range of nuclear applications, from stand-off detection of radioisotopes to forensics and safeguards.

Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE

DOE Contract Number:: AC05-76RL01830

OSTI ID:: 1574887

Report Number(s):: PNNL-SA-144962

Journal Information:: Journal of Analytical Atomic Spectrometry, Journal Name: Journal of Analytical Atomic Spectrometry Journal Issue: 11 Vol. 34

Country of Publication:: United States

Language:: English

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